Youkun Tao, Minhua Wu, Meiqi Hu, Xihua Xu, M. I. Abdullah, Jing Shao, Haijiang Wang
Hydrogen is a favored alternative to fossil fuels due to the advantages of cleanliness, zero emissions, and high calorific value. Large‐scale green hydrogen production can be achieved using proton exchange membrane water electrolyzers (PEMWEs) with utilization of renewable energy. The porous transport layer (PTL), positioned between the flow fields and catalyst layers (CLs) in PEMWEs, plays a critical role in facilitating water/gas transport, enabling electrical/thermal conduction, and mechanically supporting CLs and membranes. Superior corrosion resistance is essential as PTL operates in acidic media with oxygen saturation and high working potential. This paper covers the development of high‐performance titanium‐based PTLs for PEMWEs. The heat/electrical conduction and mass transport mechanisms of PTLs and how they affect the overall performances are reviewed. By carefully designing and controlling substrate microstructure, protective coating, and surface modification, the performance of PTL can be regulated and optimized. The two‐phase mass transport characteristics can be enhanced by fine‐tuning the microstructure and surface wettability of PTL. The addition of a microporous top‐layer can effectively improve PTL|CL contact and increase the availability of catalytic sites. The anticorrosion coatings, which are crucial for chemical stability and conductivity of the PTL, are compared and analyzed in terms of composition, fabrication, and performance.
{"title":"High‐performance porous transport layers for proton exchange membrane water electrolyzers","authors":"Youkun Tao, Minhua Wu, Meiqi Hu, Xihua Xu, M. I. Abdullah, Jing Shao, Haijiang Wang","doi":"10.1002/sus2.230","DOIUrl":"https://doi.org/10.1002/sus2.230","url":null,"abstract":"Hydrogen is a favored alternative to fossil fuels due to the advantages of cleanliness, zero emissions, and high calorific value. Large‐scale green hydrogen production can be achieved using proton exchange membrane water electrolyzers (PEMWEs) with utilization of renewable energy. The porous transport layer (PTL), positioned between the flow fields and catalyst layers (CLs) in PEMWEs, plays a critical role in facilitating water/gas transport, enabling electrical/thermal conduction, and mechanically supporting CLs and membranes. Superior corrosion resistance is essential as PTL operates in acidic media with oxygen saturation and high working potential. This paper covers the development of high‐performance titanium‐based PTLs for PEMWEs. The heat/electrical conduction and mass transport mechanisms of PTLs and how they affect the overall performances are reviewed. By carefully designing and controlling substrate microstructure, protective coating, and surface modification, the performance of PTL can be regulated and optimized. The two‐phase mass transport characteristics can be enhanced by fine‐tuning the microstructure and surface wettability of PTL. The addition of a microporous top‐layer can effectively improve PTL|CL contact and increase the availability of catalytic sites. The anticorrosion coatings, which are crucial for chemical stability and conductivity of the PTL, are compared and analyzed in terms of composition, fabrication, and performance.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":18.7,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141827709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zifan Zhang, Kun Xiang, Haitao Wang, Xin Li, J. Zou, Guijie Liang, Jizhou Jiang
Single‐atom catalysts (SACs) have rapidly become a hot topic in photocatalytic research due to their unique physical and chemical properties, high activity, and high selectivity. Among many semiconductor carriers, the special structure of carbon nitride (C3N4) perfectly meets the substrate requirements for stabilizing SACs; they can also compensate for the photocatalytic defects of C3N4 materials by modifying energy bands and electronic structures. Therefore, developing advanced C3N4‐based SACs is of great significance. In this review, we focus on elucidating efficient preparation strategies and the burgeoning photocatalytic applications of C3N4‐based SACs. We also outline prospective strategies for enhancing the performance of SACs and C3N4‐based SACs in the future. A comprehensive array of methodologies is presented for identifying and characterizing C3N4‐based SACs. This includes an exploration of potential atomic catalytic mechanisms through the simulation and regulation of atomic catalytic behaviors and the synergistic effects of single or multiple sites. Subsequently, a forward‐looking perspective is adopted to contemplate the future prospects and challenges associated with C3N4‐based SACs. This encompasses considerations, such as atomic loading, regulatory design, and the integration of machine learning techniques. It is anticipated that this review will stimulate novel insights into the synthesis of high‐load and durable SACs, thereby providing theoretical groundwork for scalable and controllable applications in the field.
{"title":"Advanced carbon nitride‐based single‐atom photocatalysts","authors":"Zifan Zhang, Kun Xiang, Haitao Wang, Xin Li, J. Zou, Guijie Liang, Jizhou Jiang","doi":"10.1002/sus2.229","DOIUrl":"https://doi.org/10.1002/sus2.229","url":null,"abstract":"Single‐atom catalysts (SACs) have rapidly become a hot topic in photocatalytic research due to their unique physical and chemical properties, high activity, and high selectivity. Among many semiconductor carriers, the special structure of carbon nitride (C3N4) perfectly meets the substrate requirements for stabilizing SACs; they can also compensate for the photocatalytic defects of C3N4 materials by modifying energy bands and electronic structures. Therefore, developing advanced C3N4‐based SACs is of great significance. In this review, we focus on elucidating efficient preparation strategies and the burgeoning photocatalytic applications of C3N4‐based SACs. We also outline prospective strategies for enhancing the performance of SACs and C3N4‐based SACs in the future. A comprehensive array of methodologies is presented for identifying and characterizing C3N4‐based SACs. This includes an exploration of potential atomic catalytic mechanisms through the simulation and regulation of atomic catalytic behaviors and the synergistic effects of single or multiple sites. Subsequently, a forward‐looking perspective is adopted to contemplate the future prospects and challenges associated with C3N4‐based SACs. This encompasses considerations, such as atomic loading, regulatory design, and the integration of machine learning techniques. It is anticipated that this review will stimulate novel insights into the synthesis of high‐load and durable SACs, thereby providing theoretical groundwork for scalable and controllable applications in the field.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":18.7,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141825814","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jianfei Wu, Ziwei Cui, Yuxuan Su, Dongfang Wu, Jundie Hu, J. Qu, Jianzhang Li, Fangyuan Kang, Dan Tian, Qichun Zhang, Yahui Cai
Developing an efficient freshwater and electricity co‐generation device (FECGD) can solve the shortage of freshwater and electricity. However, the poor salt resistance and refrigeration properties of the materials for FECGD put big challenges in the efficient and stable operation of these devices. To address these issues, we propose the covalent organic framework (COF) confined co‐polymerization strategy to prepare COF‐modified acrylamide cationic hydrogels (ACH‐COF), where hydrogen bonding interlocking between negatively charged polymer chains and COF pores can form a salt resistant hydrogel for stabilizing tunable passive interfacial cooling (TPIC). The FECPDs based on the TPIC and salt resistance of ACH‐COF display a maximum output power density of 2.28 W m−2, which is 4.3 times higher than that of a commercial thermoelectric generator under one solar radiation. The production rate of freshwater can reach 2.74 kg m−2 h−1. Our results suggest that the high efficiency and scalability of the FECGD can hold the promise of alleviating freshwater and power shortages.
{"title":"Tuning on passive interfacial cooling of covalent organic framework hydrogel for enhancing freshwater and electricity generation","authors":"Jianfei Wu, Ziwei Cui, Yuxuan Su, Dongfang Wu, Jundie Hu, J. Qu, Jianzhang Li, Fangyuan Kang, Dan Tian, Qichun Zhang, Yahui Cai","doi":"10.1002/sus2.231","DOIUrl":"https://doi.org/10.1002/sus2.231","url":null,"abstract":"Developing an efficient freshwater and electricity co‐generation device (FECGD) can solve the shortage of freshwater and electricity. However, the poor salt resistance and refrigeration properties of the materials for FECGD put big challenges in the efficient and stable operation of these devices. To address these issues, we propose the covalent organic framework (COF) confined co‐polymerization strategy to prepare COF‐modified acrylamide cationic hydrogels (ACH‐COF), where hydrogen bonding interlocking between negatively charged polymer chains and COF pores can form a salt resistant hydrogel for stabilizing tunable passive interfacial cooling (TPIC). The FECPDs based on the TPIC and salt resistance of ACH‐COF display a maximum output power density of 2.28 W m−2, which is 4.3 times higher than that of a commercial thermoelectric generator under one solar radiation. The production rate of freshwater can reach 2.74 kg m−2 h−1. Our results suggest that the high efficiency and scalability of the FECGD can hold the promise of alleviating freshwater and power shortages.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":18.7,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141828761","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electroencephalogram (EEG) is one of the most important bioelectrical signals related to brain activity and plays a crucial role in clinical medicine. Driven by continuously expanding applications, the development of EEG materials and technology has attracted considerable attention. However, systematic analysis of the sustainable development of EEG materials and technology is still lacking. This review discusses the sustainable development of EEG materials and technology. First, the developing course of EEG is introduced to reveal its significance, particularly in clinical medicine. Then, the sustainability of the EEG materials and technology is discussed from two main aspects: integrated systems and EEG electrodes. For integrated systems, sustainability has been focused on the developing trend toward mobile EEG systems and big‐data monitoring/analyzing of EEG signals. Sustainability is related to miniaturized, wireless, portable, and wearable systems that are integrated with big‐data modeling techniques. For EEG electrodes and materials, sustainability has been comprehensively analyzed from three perspectives: performance of different material/structural categories, sustainable materials for EEG electrodes, and sustainable manufacturing technologies. In addition, sustainable applications of EEG have been presented. Finally, the sustainable development of EEG materials and technology in recent decades is summarized, revealing future possible research directions as well as urgent challenges.
{"title":"Sustainable development of electroencephalography materials and technology","authors":"Ling Xiong, Nannan Li, Yiwu Luo, Lei Chen","doi":"10.1002/sus2.195","DOIUrl":"https://doi.org/10.1002/sus2.195","url":null,"abstract":"Electroencephalogram (EEG) is one of the most important bioelectrical signals related to brain activity and plays a crucial role in clinical medicine. Driven by continuously expanding applications, the development of EEG materials and technology has attracted considerable attention. However, systematic analysis of the sustainable development of EEG materials and technology is still lacking. This review discusses the sustainable development of EEG materials and technology. First, the developing course of EEG is introduced to reveal its significance, particularly in clinical medicine. Then, the sustainability of the EEG materials and technology is discussed from two main aspects: integrated systems and EEG electrodes. For integrated systems, sustainability has been focused on the developing trend toward mobile EEG systems and big‐data monitoring/analyzing of EEG signals. Sustainability is related to miniaturized, wireless, portable, and wearable systems that are integrated with big‐data modeling techniques. For EEG electrodes and materials, sustainability has been comprehensively analyzed from three perspectives: performance of different material/structural categories, sustainable materials for EEG electrodes, and sustainable manufacturing technologies. In addition, sustainable applications of EEG have been presented. Finally, the sustainable development of EEG materials and technology in recent decades is summarized, revealing future possible research directions as well as urgent challenges.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2024-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140703231","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Brenden Jing Su, J. J. Foo, Grayson Zhi Sheng Ling, Wee‐Jun Ong
Integrating H2O2 evolution with oxidative organic synthesis in a semiconductor‐driven photoredox reaction is highly attractive since H2O2 and high‐value chemicals can be concurrently produced using solar light as the only energy input. The dual‐functional photocatalytic approach, free from sacrificial agents, enables simultaneous production of H2O2 and high‐value organic chemicals. This strategy promises a green and sustainable organic synthesis with minimal greenhouse gas emissions. In this review, we first elucidate the fundamental principles of cooperative photoredox integration of H2O2 synthesis and selective organic oxidation with simultaneous utilization of photoexcited electrons and holes over semiconductor‐based photocatalysts. Afterwards, a thorough review on the recent advancements of cooperative photoredox synthesis of H2O2 and value‐added chemicals is presented. Notably, in‐depth discussions and insights into the techniques for unravelling the photoredox reaction mechanisms are elucidated. Finally, critical challenges and prospects in this thriving field are comprehensively discussed. It is envisioned that this review will serve as a pivotal guidance on the rational design of such dual‐functional photocatalytic system, thereby further stimulating the development of economical and environmentally benign H2O2 and high‐value chemicals production.
{"title":"Synergistic redox reactions toward co‐production of H2O2 and value‐added chemicals: Dual‐functional photocatalysis to achieving sustainability","authors":"Brenden Jing Su, J. J. Foo, Grayson Zhi Sheng Ling, Wee‐Jun Ong","doi":"10.1002/sus2.192","DOIUrl":"https://doi.org/10.1002/sus2.192","url":null,"abstract":"Integrating H2O2 evolution with oxidative organic synthesis in a semiconductor‐driven photoredox reaction is highly attractive since H2O2 and high‐value chemicals can be concurrently produced using solar light as the only energy input. The dual‐functional photocatalytic approach, free from sacrificial agents, enables simultaneous production of H2O2 and high‐value organic chemicals. This strategy promises a green and sustainable organic synthesis with minimal greenhouse gas emissions. In this review, we first elucidate the fundamental principles of cooperative photoredox integration of H2O2 synthesis and selective organic oxidation with simultaneous utilization of photoexcited electrons and holes over semiconductor‐based photocatalysts. Afterwards, a thorough review on the recent advancements of cooperative photoredox synthesis of H2O2 and value‐added chemicals is presented. Notably, in‐depth discussions and insights into the techniques for unravelling the photoredox reaction mechanisms are elucidated. Finally, critical challenges and prospects in this thriving field are comprehensively discussed. It is envisioned that this review will serve as a pivotal guidance on the rational design of such dual‐functional photocatalytic system, thereby further stimulating the development of economical and environmentally benign H2O2 and high‐value chemicals production.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2024-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140714286","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Re‐extracting environmentally transportable hexavalent uranium from wastewater produced by spent fuel reprocessing using the photocatalytic technology is a crucial strategy to avoid uranium pollution and recover nuclear fuel strategic resources. Here, we have designed S‐scheme 2D/0D C3N5/Fe2O3 heterojunction photocatalysts based on the built‐in electric field and the energy band bending theory, and have further revealed the immobilization process of hexavalent uranium conversion into relatively insoluble tetravalent uranium in terms of thermodynamics and kinetics. According to the results, the hexavalent uranium removal and recovery ratios in wastewater are as high as 93.38% and 83.58%, respectively. Besides, C3N5/Fe2O3 heterojunctions also exhibit satisfactory catalytic activity and selectivity even in the presence of excessive impurity cations (including Na+, K+, Ca2+, Mg2+, Sr2+, and Eu3+) or various organics (such as xylene, tributylphosphate, pyridine, tannic acid, citric acid, and oxalic acid). It is believed that this work can provide a potential opportunity for S‐scheme heterojunction photocatalysts to re‐enrich uranium from spent fuel wastewater.
利用光催化技术从乏燃料后处理产生的废水中重新提取环境可迁移的六价铀，是避免铀污染和回收核燃料战略资源的重要策略。在此，我们基于内置电场和能带弯曲理论设计了 S 型 2D/0D C3N5/Fe2O3 异质结光催化剂，并从热力学和动力学方面进一步揭示了六价铀转化为相对不溶的四价铀的固定化过程。结果表明，废水中六价铀的去除率和回收率分别高达 93.38% 和 83.58%。此外，即使在过量杂质阳离子（包括 Na+、K+、Ca2+、Mg2+、Sr2+ 和 Eu3+）或各种有机物（如二甲苯、磷酸三丁酯、吡啶、单宁酸、柠檬酸和草酸）存在的情况下，C3N5/Fe2O3 异质结也表现出令人满意的催化活性和选择性。相信这项工作能为 S 型异质结光催化剂从乏燃料废水中再富集铀提供一个潜在的机会。
{"title":"Photo‐enhanced uranium recovery from spent fuel reprocessing wastewater via S‐scheme 2D/0D C3N5/Fe2O3 heterojunctions","authors":"Qi Meng, Linzhen Wu, Xiaoyong Yang, Ying Xiong, Fanpeng Kong, Tao Duan","doi":"10.1002/sus2.199","DOIUrl":"https://doi.org/10.1002/sus2.199","url":null,"abstract":"Re‐extracting environmentally transportable hexavalent uranium from wastewater produced by spent fuel reprocessing using the photocatalytic technology is a crucial strategy to avoid uranium pollution and recover nuclear fuel strategic resources. Here, we have designed S‐scheme 2D/0D C3N5/Fe2O3 heterojunction photocatalysts based on the built‐in electric field and the energy band bending theory, and have further revealed the immobilization process of hexavalent uranium conversion into relatively insoluble tetravalent uranium in terms of thermodynamics and kinetics. According to the results, the hexavalent uranium removal and recovery ratios in wastewater are as high as 93.38% and 83.58%, respectively. Besides, C3N5/Fe2O3 heterojunctions also exhibit satisfactory catalytic activity and selectivity even in the presence of excessive impurity cations (including Na+, K+, Ca2+, Mg2+, Sr2+, and Eu3+) or various organics (such as xylene, tributylphosphate, pyridine, tannic acid, citric acid, and oxalic acid). It is believed that this work can provide a potential opportunity for S‐scheme heterojunction photocatalysts to re‐enrich uranium from spent fuel wastewater.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2024-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140778232","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jiao Lin, Xiaodong Zhang, Zhujie Li, Ersha Fan, Xiaowei Lv, Renjie Chen, Feng Wu, Li Li
Directly repairing end‐of‐life lithium‐ion battery cathodes poses significant challenges due to the diverse compositions of the wastes. Here, we propose a water‐facilitated targeted repair strategy applicable to various end‐of‐life batches and cathodes. The process involves initiating structural repair and reconstructing particle morphology in degraded LiMn2O4 (LMO) through an additional thermal drive post‐ambient water remanganization, achieving elemental repair. Compared to solid‐phase repair, the resulting LMO material exhibits superior electrochemical and kinetic characteristics. The theoretical analysis highlights the impact of Mn defects on the structural stability and electron transfer rate of degraded materials. The propensity of Mn ions to diffuse within the Mn layer, specifically occupying the Mn 16d site instead of the Li 8a site, theoretically supports the feasibility of ambient water remanganization. Moreover, this method proves effective in the relithiation of degraded layered cathode materials, yielding single crystals. By combining low energy consumption, environmental friendliness, and recyclability, our study proposes a sustainable approach to utilizing spent batteries. This strategy holds the potential to enable the industrial direct repair of deteriorated cathode materials.
{"title":"Water‐facilitated targeted repair of degraded cathodes for sustainable lithium‐ion batteries","authors":"Jiao Lin, Xiaodong Zhang, Zhujie Li, Ersha Fan, Xiaowei Lv, Renjie Chen, Feng Wu, Li Li","doi":"10.1002/sus2.194","DOIUrl":"https://doi.org/10.1002/sus2.194","url":null,"abstract":"Directly repairing end‐of‐life lithium‐ion battery cathodes poses significant challenges due to the diverse compositions of the wastes. Here, we propose a water‐facilitated targeted repair strategy applicable to various end‐of‐life batches and cathodes. The process involves initiating structural repair and reconstructing particle morphology in degraded LiMn2O4 (LMO) through an additional thermal drive post‐ambient water remanganization, achieving elemental repair. Compared to solid‐phase repair, the resulting LMO material exhibits superior electrochemical and kinetic characteristics. The theoretical analysis highlights the impact of Mn defects on the structural stability and electron transfer rate of degraded materials. The propensity of Mn ions to diffuse within the Mn layer, specifically occupying the Mn 16d site instead of the Li 8a site, theoretically supports the feasibility of ambient water remanganization. Moreover, this method proves effective in the relithiation of degraded layered cathode materials, yielding single crystals. By combining low energy consumption, environmental friendliness, and recyclability, our study proposes a sustainable approach to utilizing spent batteries. This strategy holds the potential to enable the industrial direct repair of deteriorated cathode materials.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2024-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140221621","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zheng Zhang, Danyang Li, Yunchuan Tu, Jiao Deng, Huiting Bi, Yongchao Yao, Yan Wang, Tingshuai Li, Yongsong Luo, Shengjun Sun, D. Zheng, S. Carabineiro, Zhou Chen, Junjiang Zhu, Xuping Sun
The electrocatalytic synthesis of C–N coupling compounds from CO2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality and reduce environmental pollution, but also establishes a route to synthesize valuable chemicals, such as urea, amide, and amine. This innovative approach expands the application range and product categories beyond simple carbonaceous species in electrocatalytic CO2 reduction, which is becoming a rapidly advancing field. This review summarizes the research progress in electrocatalytic urea synthesis, using N2, NO2−, and NO3− as nitrogenous species, and explores emerging trends in the electrosynthesis of amide and amine from CO2 and nitrogen species. Additionally, the future opportunities in this field are highlighted, including electrosynthesis of amino acids and other compounds containing C–N bonds, anodic C–N coupling reactions beyond water oxidation, and the catalytic mechanism of corresponding reactions. This critical review also captures the insights aimed at accelerating the development of electrochemical C–N coupling reactions, confirming the superiority of this electrochemical method over the traditional techniques.
{"title":"Electrocatalytic synthesis of C–N coupling compounds from CO2 and nitrogenous species","authors":"Zheng Zhang, Danyang Li, Yunchuan Tu, Jiao Deng, Huiting Bi, Yongchao Yao, Yan Wang, Tingshuai Li, Yongsong Luo, Shengjun Sun, D. Zheng, S. Carabineiro, Zhou Chen, Junjiang Zhu, Xuping Sun","doi":"10.1002/sus2.193","DOIUrl":"https://doi.org/10.1002/sus2.193","url":null,"abstract":"The electrocatalytic synthesis of C–N coupling compounds from CO2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality and reduce environmental pollution, but also establishes a route to synthesize valuable chemicals, such as urea, amide, and amine. This innovative approach expands the application range and product categories beyond simple carbonaceous species in electrocatalytic CO2 reduction, which is becoming a rapidly advancing field. This review summarizes the research progress in electrocatalytic urea synthesis, using N2, NO2−, and NO3− as nitrogenous species, and explores emerging trends in the electrosynthesis of amide and amine from CO2 and nitrogen species. Additionally, the future opportunities in this field are highlighted, including electrosynthesis of amino acids and other compounds containing C–N bonds, anodic C–N coupling reactions beyond water oxidation, and the catalytic mechanism of corresponding reactions. This critical review also captures the insights aimed at accelerating the development of electrochemical C–N coupling reactions, confirming the superiority of this electrochemical method over the traditional techniques.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2024-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140250793","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A 3D nanostructured scaffold as the host for zinc enables effective inhibition of anodic dendrite growth. However, the increased electrode/electrolyte interface area provided by using 3D matrices exacerbates the passivation and localized corrosion of the Zn anode, ultimately bringing about the degradation of the electrochemical performance. Herein, a nanoscale coating of inorganic–organic hybrid (α‐In2Se3‐Nafion) onto a flexible carbon nanotubes (CNTs) framework (ISNF@CNTs) is designed as a Zn plating/stripping scaffold to ensure uniform Zn nucleation, thus achieving a dendrite‐free and durable Zn anode. The introduced inorganic–organic interfacial layer is dense and sturdy, which hinders the direct exposure of deposited Zn to electrolytes and mitigates the side reactions. Meanwhile, the zincophilic nature of ISNF can largely reduce the nucleation energy barrier and promote the ion‐diffusion transportation. Consequently, the ISNF@CNTs@Zn electrode exhibits a low‐voltage hysteresis and a superior cycling life (over 1500 h), with dendrite‐free Zn‐plating behaviors in a typical symmetrical cell test. Additionally, the superior feature of ISNF@CNTs@Zn anode is further demonstrated by Zn‐MnO2 cells in both coin and flexible quasi‐solid‐state configurations. This work puts forward an inspired remedy for advanced Zn‐ion batteries.
{"title":"Dendrite‐free Zn deposition initiated by nanoscale inorganic–organic coating‐modified 3D host for stable Zn‐ion battery","authors":"Jiaming Dong, Junwen Duan, Ruirui Cao, Wang Zhang, Kangkang Fang, Hao Yang, Ying Liu, Zhitao Shen, Fumin Li, Rong Liu, Mengqi Jin, Longhui Lei, Huilin Li, Chong Chen","doi":"10.1002/sus2.189","DOIUrl":"https://doi.org/10.1002/sus2.189","url":null,"abstract":"A 3D nanostructured scaffold as the host for zinc enables effective inhibition of anodic dendrite growth. However, the increased electrode/electrolyte interface area provided by using 3D matrices exacerbates the passivation and localized corrosion of the Zn anode, ultimately bringing about the degradation of the electrochemical performance. Herein, a nanoscale coating of inorganic–organic hybrid (α‐In2Se3‐Nafion) onto a flexible carbon nanotubes (CNTs) framework (ISNF@CNTs) is designed as a Zn plating/stripping scaffold to ensure uniform Zn nucleation, thus achieving a dendrite‐free and durable Zn anode. The introduced inorganic–organic interfacial layer is dense and sturdy, which hinders the direct exposure of deposited Zn to electrolytes and mitigates the side reactions. Meanwhile, the zincophilic nature of ISNF can largely reduce the nucleation energy barrier and promote the ion‐diffusion transportation. Consequently, the ISNF@CNTs@Zn electrode exhibits a low‐voltage hysteresis and a superior cycling life (over 1500 h), with dendrite‐free Zn‐plating behaviors in a typical symmetrical cell test. Additionally, the superior feature of ISNF@CNTs@Zn anode is further demonstrated by Zn‐MnO2 cells in both coin and flexible quasi‐solid‐state configurations. This work puts forward an inspired remedy for advanced Zn‐ion batteries.","PeriodicalId":29781,"journal":{"name":"SusMat","volume":null,"pages":null},"PeriodicalIF":28.4,"publicationDate":"2024-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140266496","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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